Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystals

Daofu Wu; Xiaoqing Liu; Changqing Tian; Jinchen Zhou; Junan Lai; Hongmei Ran; Bo Gao; Miao Zhou; Qiang Huang; Xiaosheng Tang

doi:10.1016/j.isci.2023.107355

Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs₂AgSbCl₆ double perovskite microcrystals

Daofu Wu
, Xiaoqing Liu
, Changqing Tian
, Jinchen Zhou
, Junan Lai
, Hongmei Ran
, Bo Gao
, Miao Zhou^*
, Qiang Huang^*
, Xiaosheng Tang^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

10 Scopus citations

Abstract

Lead halide perovskites are prospective candidates for CO₂ photoconversion. Herein, we report copper-doped lead-free Cs₂AgSbCl₆ double perovskite microcrystals (MCs) for gas-solid phase photocatalytic CO₂ reduction. The 0.2Cu@Cs₂AgSbCl₆ double perovskite MCs display unprecedented CO₂ photoreduction capability with CO and CH₄ yields of 412 and 128 μmol g⁻¹, respectively. The ultrafast transient absorption spectroscopy reveals the enhanced separation of photoexcited carriers in copper-doped Cs₂AgSbCl₆ MCs. The active sites and reaction intermediates on the surface of the doped Cs₂AgSbCl₆ are dynamically monitored and precisely unraveled based on the in-situ Fourier transform infrared spectroscopy investigation. In combination with density functional theory calculations, it is revealed that the copper-doped Cs₂AgSbCl₆ MCs facilitate sturdy CO₂ adsorption and activation and strikingly enhance the photocatalytic performance. This work offers an in-depth interpretation of the photocatalytic mechanism of Cs₂AgSbCl₆ doped with copper, which may provide guidance for future design of high-performance photocatalysts for solar fuel production.

Original language	English
Article number	107355
Journal	iScience
Volume	26
Issue number	8
DOIs	https://doi.org/10.1016/j.isci.2023.107355
State	Published - 18 Aug 2023
Externally published	Yes

Keywords

Chemical property
Materials property
Optical materials

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10.1016/j.isci.2023.107355

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@article{367ebfc6a8b04162bad9631d25f28732,

title = "Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystals",

abstract = "Lead halide perovskites are prospective candidates for CO2 photoconversion. Herein, we report copper-doped lead-free Cs2AgSbCl6 double perovskite microcrystals (MCs) for gas-solid phase photocatalytic CO2 reduction. The 0.2Cu@Cs2AgSbCl6 double perovskite MCs display unprecedented CO2 photoreduction capability with CO and CH4 yields of 412 and 128 μmol g−1, respectively. The ultrafast transient absorption spectroscopy reveals the enhanced separation of photoexcited carriers in copper-doped Cs2AgSbCl6 MCs. The active sites and reaction intermediates on the surface of the doped Cs2AgSbCl6 are dynamically monitored and precisely unraveled based on the in-situ Fourier transform infrared spectroscopy investigation. In combination with density functional theory calculations, it is revealed that the copper-doped Cs2AgSbCl6 MCs facilitate sturdy CO2 adsorption and activation and strikingly enhance the photocatalytic performance. This work offers an in-depth interpretation of the photocatalytic mechanism of Cs2AgSbCl6 doped with copper, which may provide guidance for future design of high-performance photocatalysts for solar fuel production.",

keywords = "Chemical property, Materials property, Optical materials",

author = "Daofu Wu and Xiaoqing Liu and Changqing Tian and Jinchen Zhou and Junan Lai and Hongmei Ran and Bo Gao and Miao Zhou and Qiang Huang and Xiaosheng Tang",

note = "Publisher Copyright: {\textcopyright} 2023 The Authors",

year = "2023",

month = aug,

day = "18",

doi = "10.1016/j.isci.2023.107355",

language = "英语",

volume = "26",

journal = "iScience",

issn = "2589-0042",

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TY - JOUR

T1 - Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystals

AU - Wu, Daofu

AU - Liu, Xiaoqing

AU - Tian, Changqing

AU - Zhou, Jinchen

AU - Lai, Junan

AU - Ran, Hongmei

AU - Gao, Bo

AU - Zhou, Miao

AU - Huang, Qiang

AU - Tang, Xiaosheng

PY - 2023/8/18

Y1 - 2023/8/18

N2 - Lead halide perovskites are prospective candidates for CO2 photoconversion. Herein, we report copper-doped lead-free Cs2AgSbCl6 double perovskite microcrystals (MCs) for gas-solid phase photocatalytic CO2 reduction. The 0.2Cu@Cs2AgSbCl6 double perovskite MCs display unprecedented CO2 photoreduction capability with CO and CH4 yields of 412 and 128 μmol g−1, respectively. The ultrafast transient absorption spectroscopy reveals the enhanced separation of photoexcited carriers in copper-doped Cs2AgSbCl6 MCs. The active sites and reaction intermediates on the surface of the doped Cs2AgSbCl6 are dynamically monitored and precisely unraveled based on the in-situ Fourier transform infrared spectroscopy investigation. In combination with density functional theory calculations, it is revealed that the copper-doped Cs2AgSbCl6 MCs facilitate sturdy CO2 adsorption and activation and strikingly enhance the photocatalytic performance. This work offers an in-depth interpretation of the photocatalytic mechanism of Cs2AgSbCl6 doped with copper, which may provide guidance for future design of high-performance photocatalysts for solar fuel production.

AB - Lead halide perovskites are prospective candidates for CO2 photoconversion. Herein, we report copper-doped lead-free Cs2AgSbCl6 double perovskite microcrystals (MCs) for gas-solid phase photocatalytic CO2 reduction. The 0.2Cu@Cs2AgSbCl6 double perovskite MCs display unprecedented CO2 photoreduction capability with CO and CH4 yields of 412 and 128 μmol g−1, respectively. The ultrafast transient absorption spectroscopy reveals the enhanced separation of photoexcited carriers in copper-doped Cs2AgSbCl6 MCs. The active sites and reaction intermediates on the surface of the doped Cs2AgSbCl6 are dynamically monitored and precisely unraveled based on the in-situ Fourier transform infrared spectroscopy investigation. In combination with density functional theory calculations, it is revealed that the copper-doped Cs2AgSbCl6 MCs facilitate sturdy CO2 adsorption and activation and strikingly enhance the photocatalytic performance. This work offers an in-depth interpretation of the photocatalytic mechanism of Cs2AgSbCl6 doped with copper, which may provide guidance for future design of high-performance photocatalysts for solar fuel production.

KW - Chemical property

KW - Materials property

KW - Optical materials

UR - https://www.scopus.com/pages/publications/85165347414

U2 - 10.1016/j.isci.2023.107355

DO - 10.1016/j.isci.2023.107355

M3 - 文章

AN - SCOPUS:85165347414

SN - 2589-0042

VL - 26

JO - iScience

JF - iScience

IS - 8

M1 - 107355

ER -

Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs₂AgSbCl₆ double perovskite microcrystals

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